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Gating Single-Molecule Fluorescence with Electrons

Katharina Kaiser1,2,*, Song Jiang1, Michelangelo Romeo1, Fabrice Scheurer1, Guillaume Schull1,†, and Anna Rosławska1,3,‡

  • *Contact author: katharina.kaiser@uni-goettingen.de
  • †Contact author: guillaume.schull@ipcms.unistra.fr
  • ‡Contact author: a.roslawska@fkf.mpg.de
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Phys. Rev. Lett. 133, 156902 – Published 8 October, 2024

DOI: https://doi.org/10.1103/PhysRevLett.133.156902

Abstract

Tip-enhanced photoluminescence (TEPL) measurements are performed with subnanometer spatial resolution on individual molecules decoupled from a metallic substrate by a thin NaCl layer. TEPL spectra reveal progressive fluorescence quenching with decreasing tip-molecule distance when electrons tunneling from the tip of a scanning tunneling microscope are injected at resonance with the molecular states. Rate equations based on a many-body model reveal that the luminescence quenching is due to a progressive population inversion between the ground neutral (S0) and the ground charge (D0−) states of the molecule occurring when the current is raised. We demonstrate that the bias voltage and the lateral tip position can be used to gate the molecular emission. Our approach can be applied to any molecular system, providing unprecedented control over the fluorescence of a single molecule.

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Phys. Rev. Lett. 133, 156902– Published 8 October, 2024
  • Received 18 March 2024
  • Revised 4 July 2024
  • Accepted 10 September 2024
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI. Open access publication funded by the Max Planck Society.

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